The creation of anticorrosion hybrid zinc-based coatings containing chitosan particles with low (LMC) or high (HMC) molecular weight is an effective method for safe and durable exploitation of different steel infrastructures. In this work, hybrid coatings consisting of zinc and two types of chitosan particles (LMC or HMC) were obtained to protect low-carbon steel from corrosion attack in a chloride environment. Chitosans with different molecular weights (CS50 Mw 50–190 kDa and CS190 Mw 190–310 kDa) have been applied. Furthermore, both particle types were prepared with or without additional content of incorporated corrosion inhibitor benzotriazole (BTA). The chitosan particles were obtained and thereafter electrodeposited in the form of hybrid coatings on mild steel substrates. The electrokinetic charge and hydrodynamic size of the particles and the stability of their aqueous suspensions were evaluated using dynamic light scattering. The concentration of BTA loaded into the particles was determined by the difference between the initial concentration of the compound added during the particle preparation and the concentration in the supernatant after centrifugation of the dispersion. The hybrid coatings were compared concerning their surface morphology, topography, and hydrophilicity (SEM and AFM analysis, water contact angle measurement) as well as corrosion and electrochemical behavior (potentiodynamic polarization curves—PD, polarization resistance—Rp, cyclic voltammetry—CVA). The protective characteristics of the coatings were studied in 5% NaCl solution. The results obtained from the PD studies demonstrated lower corrosion current densities of all hybrid coatings compared to the ordinary zinc one. In addition, the Rp tests showed enhanced protective ability and corrosion resistance of LMC and LMCB compared to the ordinary zinc, HMC, and HMCB, respectively. The obtained scientific information presented the effect of the molecular weight and ζ-potential of the particles on the anticorrosion ability of the hybrid coatings compared to the ordinary zinc one.